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0D Hybrid Zn/Cd Halied for Color-Time-Dual-Resolved Security Applications: We devise a family of zero-dimensional (0D) hybrid metal halides based RTP materials with dual phosphorescence performance and adjustable lifetime scale, which realize color-lifetime-dual-resolved encoding ability, showcasing potential applications in multilevel anti-counterfeiting and information security. [Display omitted] • A new optical multiplexing concept of simultaneously utilizing the varied emission color and lifetime as dual temporary codes was proposed. • A new family of zero-dimensional (0D) organic metal halides was directly synthesized accompanied by tailorable lifetime at the same molecular platform. • High-security anti-Counterfeiting and 4D information encryption-decryption were demonstrated. Luminescent materials with engineered optical properties play an important role in anti-counterfeiting and information security technology. However, conventional luminescent coding is limited by fluorescence color or intensity, and high-level multi-dimensional luminescent encryption technology remains a critically challenging goal in different scenarios. To improve the encoding capacity, we present an optical multiplexing concept by synchronously manipulating the emission color and decay lifetimes of room-temperature phosphorescence materials at molecular level. Herein, we devise a family of zero-dimensional (0D) hybrid metal halides by combining organic phosphonium cations and metal halide tetrahedral anions as independent luminescent centers, which display blue phosphorescence and green persistent afterglow with the highest quantum yields of 39.9 % and 57.3 %, respectively. Significantly, the luminescence lifetime can be fine-tuned in the range of 0.0968–0.5046 μs and 33.46–125.61 ms as temporary time coding through precisely controlling the heavy atomic effect and inter-molecular interactions. As a consequence, synchronous blue phosphorescence and green afterglow are integrated into one 0D halide platform with adjustable emission lifetime acting as color- and time-resolved dual RTP materials, which realize the multiple applications in high-level anti-counterfeiting and information storage. The color-lifetime-dual-resolved encoding ability greatly broadens the scope of luminescent halide materials for optical multiplexing applications. [ABSTRACT FROM AUTHOR]

Zero‐dimensional (0D) hybrid metal halides have been emerged as room‐temperature phosphorescence (RTP) materials, but synchronous optimization of multiple phosphorescence performance in one structural platform remains less resolved, and stable RTP activity in aqueous medium is also unrealized due to serious instability toward water and oxygen. Herein, we demonstrated a photophysical tuning strategy in a new 0D hybrid zinc halide family of (BTPP)2ZnX4 (BTPP=benzyltriphenylphosphonium, X=Cl and Br). Infrequently, the delicate combination of organic and inorganic species enables this family to display multiple ultralong green afterglow and efficient self‐trapped exciton (STE) associated cyan phosphorescence. Compared with inert luminescence of [BTPP]+ cation, incorporation of anionic [ZnX4]2− effectively enhance the spin‐orbit coupling effect, which significantly boosts the photoluminescence quantum yield (PLQY) up to 30.66 % and 54.62 % for afterglow and phosphorescence, respectively. Synchronously, the corresponding luminescence lifetime extend to 143.94 ms and 0.308 μs surpassing the indiscernible phosphorescence of [BTPP]X salt. More importantly, this halide family presents robust RTP emission with nearly unattenuated PLQY in water and harsh condition (acid and basic aqueous solution) over half a year. The highly efficient integrated afterglow and STE phosphorescence as well as ultrahigh aqueous state RTP realize multiple anti‐counterfeiting applications in wide chemical environments. [ABSTRACT FROM AUTHOR]